Alloying metal cations in perovskite nanocrystals is a new route to controlling hot carrier cooling

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Abstract

Hot carrier cooling is slowed down upon alloying tin in lead-halide perovskite nanocrystals through the engineering of carrier-phonon and carrier-defect interactions.

Abstract

The key electronic and phononic processes governing hot carrier cooling dynamics in perovskite nanosystems can be tuned through Pb-Sn alloying.

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Most cited references 24

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Observation of a hot-phonon bottleneck in lead-iodide perovskites

Ye Yang, David Ostrowski, Ryan M. France … (2016)

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Screening in crystalline liquids protects energetic carriers in hybrid perovskites.

Haiming Zhu, Kiyoshi Miyata, Yongping Fu … (2016)

Hybrid lead halide perovskites exhibit carrier properties that resemble those of pristine nonpolar semiconductors despite static and dynamic disorder, but how carriers are protected from efficient scattering with charged defects and optical phonons is unknown. Here, we reveal the carrier protection mechanism by comparing three single-crystal lead bromide perovskites: CH3NH3PbBr3, CH(NH2)2PbBr3, and CsPbBr3 We observed hot fluorescence emission from energetic carriers with ~10(2)-picosecond lifetimes in CH3NH3PbBr3 or CH(NH2)2PbBr3, but not in CsPbBr3 The hot fluorescence is correlated with liquid-like molecular reorientational motions, suggesting that dynamic screening protects energetic carriers via solvation or large polaron formation on time scales competitive with that of ultrafast cooling. Similar protections likely exist for band-edge carriers. The long-lived energetic carriers may enable hot-carrier solar cells with efficiencies exceeding the Shockley-Queisser limit.

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Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy.

Kai Zhu, Zhi Hong GUO, Yan Wan … (2017)

The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 picoseconds was observed in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. We report direct visualization of hot-carrier migration in methylammonium lead iodide (CH3NH3PbI3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was observed to correlate with excess kinetic energy, resulting in up to 230 nanometers transport distance that could overcome grain boundaries. The nonequilibrium transport persisted over tens of picoseconds and ~600 nanometers before reaching the diffusive transport limit. These results suggest potential applications of hot-carrier devices based on hybrid perovskites.

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Author and article information

Contributors

Artem A. Bakulin:

ORCID: http://orcid.org/0000-0002-3998-2000

a.bakulin@imperial.ac.uk

Journal

Journal ID (nlm-ta): Light Sci Appl

Journal ID (iso-abbrev): Light Sci Appl

Title: Light, Science & Applications

Publisher: Nature Publishing Group UK (London )

ISSN (Print): 2095-5545

ISSN (Electronic): 2047-7538

Publication date (Electronic): 20 November 2023

Publication date PMC-release: 20 November 2023

Publication date Collection: 2023

Volume: 12

Electronic Location Identifier: 276

Affiliations

Department of Chemistry and Centre for Processable Electronics, Imperial College London, ( https://ror.org/041kmwe10) London, W12 0BZ UK

Author information

Navendu Mondal http://orcid.org/0000-0001-5002-9678

Ben P. Carwithen http://orcid.org/0000-0002-3140-1793

Artem A. Bakulin http://orcid.org/0000-0002-3998-2000

Article

Publisher ID: 1316

DOI: 10.1038/s41377-023-01316-x

PMC ID: 10662473

PubMed ID: 37985751

SO-VID: 8dd8a95a-d94c-4cc2-b5cb-545be031293f

License:

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

History

Funding

Funded by: FundRef https://doi.org/10.13039/501100000780, European Commission (EC);

Award ID: H2020-MSCA-IF-2020-101018002

Award Recipient : Navendu Mondal

Custom metadata

Keywords: ultrafast photonics,nanoparticles,optical spectroscopy

Data availability:

Keywords: ultrafast photonics, nanoparticles, optical spectroscopy

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